Abstract

This study is to improve understanding of nonlinear optics through investigating the microstructures of carbon disulfide (CS2) liquid, an important nonlinear optical material. First principles methods are employed in this work to investigate the structure, vibrational spectra, and the 2nd hyperpolarizabilites of CS2clusters up to tetramers. Three types of molecular arrangements of clusters with different sizes are identified. The clusterconformations are prone to inter-converting under external disturbance due to the weak interactions among molecules. The correlation between the nonlinear optical properties and the conformation of CS2clusters are studied in detail in this work.

Received 25 May 2012Accepted 14 August 2012Published online 31 August 2012

Acknowledgments:

This work was supported by Nature Science Foundation of China (11104048), the State Key Lab of Urban Water Resource and Environment (HIT) (2012DX02), National Key Laboratory of Materials Behaviors and Evaluation Technology in Space Environments (HIT), and the Open Project of State Key Laboratory of Supramolecular Structure and Materials (SKLSSM 201206).